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Low carbon alcohol fuel electrolysis of hydrogen generation catalyzed by a novel and effective Pt–CoTe/C bifunctional catalyst system

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Green Energy & Environment 2024年第4期9卷 758-770页

作者： Yang Zhou Lice Yu Jinfa Chang ligang feng Jiujun Zhang School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou225002JiangsuChina NanoScience Technology Center University of Central FloridaOrlandoFL32826USA College of Sciences&Institute for Sustainable Energy Shanghai UniversityShanghai200444China

Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions.Herein,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation.Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol electrolysis.Moreover,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique.The high catalytic kinetics and stability,as well as the promotion effect,were also carefully discussed.Specifically,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.

关键词： Methanol electrolysis Ethanol electrolysis Cobalt telluride Pt-based electrocatalyst Hydrogen evolution reaction

Fully fluorinated hybrid zeolite imidazole/Prussian blue analogs with combined advantages for efficient oxygen evolution reaction

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Chinese Chemical Letters 2024年第6期35卷 222-228页

作者： Jiayu Xu Meng Li Baoxia Dong ligang feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

Hybrid metal-organic framework(MOF)derivatives play a significant role in the novel catalyst development in energy conversion reactions.Here,we demonstrated the low-temperature fully fluorinated zeolitic imidazole framework(ZIF)coupled with a three-dimensional open framework Prussian blue analog(PBA)with combined advantages for electrocatalytic oxygen evolution reaction(OER)in water splitting reaction.The spectroscopic analysis and the electrochemical studies revealed the combined advantages of efficient electronic effect and active site synergism.Because of good conductivity improvement by Ndoped carbon derived from ZIF and the high electrochemical surface area and active site exposure from PBA derivatives,good catalytic performance was obtained on the optimal catalyst of Co Ni ZIF/Co Fe-PBAF-300,which required a low overpotential of 250 m V to reach 10 m A/cm^(2)loaded on the glassy carbon electrode,with Tafel slope of 47.4 m V/dec,and very high dynamic and steady stability.In addition,the multi-component with the mixed structure from highly polar metal fluorides promoted the easy formation of the active phase as revealed by the post-sample analysis.The current results showed a novel composite catalyst materials development from the hybrid MOF derivatives,which would be promising in the electrolysis of water oxidation reactions and energy-relevant catalysis reactions.

关键词： Metal-organic framework Zeolitic imidazole framework Prussian blue analog Fluoridation Multi-component Oxygen evolution reaction

Au nanoclusters anchored on TiO_(2) nanosheets for high-efficiency electroreduction of nitrate to ammonia

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Nano Research 2024年第3期17卷 1209-1216页

作者： Miaosen Yang Tianran Wei Jia He Qian Liu ligang feng Hongyi Li Jun Luo Xijun Liu School of Chemical Engineering Northeast Electric Power UniversityJilin 132012China Nanchang Institute of Technology Nanchang 330044China State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830017China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China Institute for New Energy Materials and Low-Carbon Technologies School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China Institute for Advanced Study Chengdu UniversityChengdu 610106China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China Guangzhou Panyu Polytechnic Guangzhou 511483China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaLonghua DistrictShenzhen 518110China

Electrocatalytic nitrate reduction reaction(NO_(3)RR)offers a unique rationale for green NH_(3) synthesis,yet the lack of high-efficiency NO_(3)RR catalysts remains a great challenge.In this work,we show that Au nanoclusters anchored on TiO_(2) nanosheets can efficiently catalyze the conversion of NO_(3)RR-to-NH_(3) under ambient conditions,achieving a maximal Faradic efficiency of 91%,a peak yield rate of 1923μg·h^(-1)·mgcat.-1,and high durability over 10 consecutive cycles,all of which are comparable to the recently reported metrics(including transition metal and noble metal-based catalysts)and exceed those of pristine TiO_(2).Moreover,a galvanic Zn-nitrate battery using the catalyst as the cathode was proposed,which shows a power density of 3.62 mW·cm^(-2) and a yield rate of 452μg·h^(-1)·mgcat.-1.Theoretical simulations further indicate that the atomically dispersed Au clusters can promote the adsorption and activation of NO_(3)-species,and reduce the NO_(3)RR-to-NH_(3) barrier,thus leading to an accelerated cathodic reaction.This work highlights the importance of metal clusters for the NH_(3) electrosynthesis and nitrate removal.

关键词： NH3 electrosynthesis Zn-nitrate battery Au nanoclusters nitrate reduction reaction(NRR) TiO_(2)nanosheets

Coupling Co-Ni phosphides for energy-saving alkaline seawater splitting

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Nano Research 2024年第6期17卷 4797-4806页

作者： Weijia Liu Wenxian Liu Tong Hou Junyang Ding Zhigui Wang Ruilian Yin Xingyuan San ligang feng Jun Luo Xijun Liu State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Nonferrous Metals and Featured MaterialsMOE Key Laboratory of New Processing Technology for Nonferrous Metals and MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China Hebei Key Laboratory of Optic-electronic Information and Materials the College of Physics Science and TechnologyHebei UniversityBaoding 071002China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

The coupling of energy-saving small molecule conversion reactions and hydrogen evolution reaction(HER)in seawater electrolytes can reduce the energy consumption of seawater electrolysis and mitigate chlorine corrosion issues.However,the fabrication of efficient multifunctional catalysts for this promising technology is of great challenge.Herein,a heterostructured catalyst comprising CoP and Ni_(2)P on nickel foam(CoP/Ni_(2)P@NF)is reported for hydrazine oxidation(HzOR)-assisted alkaline seawater splitting.The coupling of CoP and Ni_(2)P optimizes the electronic structure of the active sites and endows excellent electrocatalytic performance for HzOR and HER.Impressively,the two-electrode HzOR-assisted alkaline seawater splitting(OHzS)cell based on the CoP/Ni_(2)P@NF required only 0.108 V to deliver 100 mA·cm^(−2),much lower than 1.695 V for alkaline seawater electrolysis cells.Moreover,the OHzS cell exhibits satisfactory stability over 48 h at a high current density of 500 mA·cm^(−2).Furthermore,the CoP/Ni_(2)P@NF heterostructured catalyst also efficiently catalyzed glucose oxidation,methanol oxidation,and urea oxidation in alkaline seawater electrolytes.This work paves a path for high-performance heterostructured catalyst preparation for energy-saving seawater electrolysis for H_(2) production.

关键词： seawater splitting heterostructure electrocatalysis hydrazine oxidation reaction hydrogen evolution reaction

Phase and chemical state tuning of FeNi oxides for oxygen evolution reaction

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Science China Chemistry 2024年第8期 2755-2766页

作者： Jiawei Wu Zhouyang Ma Lice Yu Shuli Wang Fulin Yang ligang feng School of Chemistry and Chemical Engineering Yangzhou University

Advancing and deploying the Fe Ni-based catalyst, the state-of-the-art pre-electrocatalysts, for oxygen evolution reactions（OER）still suffer from unclear chemical state correlation to the catalytic ability, as evidenced by the variedly reported performance for the different Fe Ni structures. Herein, we contributed the phase and redox chemical states tuning of Fe Ni oxides by the surface microenvironment regulation for the OER catalysis that was realized by the urea-assisted pyrolysis and molybdenum-doping technique by integrating molybdenum into the iron–nickel metal-organic precursor. Driven by the complicated and compromised atmosphere, namely, the oxidation state driven by the Mo doping and reduction ability induced by the urea-assisted pyrolysis,could transfer confined Fe Ni oxides to hybrid phases of Fe2O3and FeNi3alloy, and the resultant compromised chemical states by the charge redistribution imparted very high electrocatalytic performance for OER compared with the control samples. The insitu Raman spectroscopy and post-XPS analysis confirmed the facile Fe/Ni oxyhydroxide active phase formation resulting from the proper phase and chemical states, and theoretical analysis disclosed the microenvironment regulation resulting in the charge redistribution forming the electron accumulation and depletion sites to accelerate the oxygen-species to oxyhydroxide-species transformation and enhance the electronic state density near the Fermi level by significantly reducing the energy barrier. The work not only showed the importance of surface chemical state tunning that can basically answer the varied performance of Fe Ni catalysts but also revealed an effective approach for fine-tuning their catalytic properties.

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Resilient sliding mode control for 2D CPSs under denial-of-service attacks

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Science China(Information Sciences) 2024年第6期67卷 262-278页

作者： Lingling LI Rongni YANG Zhiguang feng ligang WU College of Intelligent Systems Science and Engineering Harbin Engineering University School of Control Science and Engineering Shandong University School of Astronautics Harbin Institute of Technology

This study addresses the resilient sliding mode control(SMC) problem for two-dimensional cyber-physical systems(2D CPSs) characterized by the Roesser model under denial-of-service attack(DoSA), which can interfere with signal transmission over the communication network. First, the DoS-A model is established by introducing constraints on the Do S frequency and duration. Then, based on active or silent attack situations, the considered system is described as a switched mode. Furthermore, together with Lyapunov theory, the average dwell time technique is employed to deduce sufficient criteria that assure the existence of the desired sliding mode controller. Finally, verification examples are provided to show the validity of the established SMC scheme.

关键词： two-dimensional systems cyber-physical systems denial-of-service attack resilient sliding mode control

NiSe_(2)-CoSe_(2) with a Hybrid Nanorods and Nanoparticles Structure for Efficient Oxygen Evolution Reaction

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Chinese Journal of Structural Chemistry 2022年第1期41卷 19-24页

作者： Meng Li ligang feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2) consisting of nanorods and nanoparticles for the efficient OER in the alkaline electrolyte.This catalyst system can be easily fabricated via a low-temperature selenization of the solvothermal synthesized NiCo(OH)x precursor and the unique morphology of hybrid nanorods and nanoparticles was found by the electron microscopy analysis.The high valence state of the metal species was indicated by X-ray photoelectron spectroscopy study and a strong electronic effect was found in the NiSe_(2)-CoSe_(2) catalyst system compared to their counterparts.As a result,NiSe_(2)-CoSe_(2) exhibited high catalytic performance with a low overpotential of 250 mV to reach 10 mA·cm^(-2) for OER in the alkaline solution.Furthermore,high catalytic stability and catalytic kinetics were also observed.The superior performance can be attributed to the high valence states of Ni and Co and their strong synergetic coupling effect between the nanorods and nanoparticles,which could accelerate the charge transfer and offer abundant electrocatalytic active sites.The current work offers an efficient hetero-structure catalyst system for OER,and the results are helpful for the catalysis understanding.

关键词： oxygen evolution reaction NiSe_(2) CoSe_(2) hetero-structure electrocatalysis

Advances in anode catalysts of methanol-assisted water-splitting reactions for hydrogen generation

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Chinese Journal of Structural Chemistry 2023年第10期42卷 54-66页

作者： Chunru Liu ligang feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou225002PR China

Methanol-assisted water-splitting reaction for green hydrogen generation is more competitive to the traditional water electrolysis driven by sustainable energies due to the largely reduced energy costs.Increasing attention currently is directed to the highly efficient methanol electrooxidation catalysts that determine the catalysis efficiency,and some advanced catalysts have been developed.Given the significant advances,this review proposed a summary of the recent progress in catalysts for methanol-assisted water electrolysis.The mechanism of methanol-assisted water-splitting reaction classified by noble and non-noble metals was first presented by taking into account their distinct redox reactions.Then,the research progress of these catalysts for methanol-assisted water-splitting reactions is summarized and discussed,and the challenges and problems associated with catalyst design and optimization as well as their practical application were finally commented on.This review would be a valuable reference for catalyst development and mechanism understanding in methanol-assisted water-splitting reactions for hydrogen generation.

关键词： Electrocatalysis Methanol oxidation reaction Water splitting Hydrogen generation

Advances of PtRu-Based Electrocatalysts for Methanol Oxidation

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Chinese Journal of Structural Chemistry 2022年第7期41卷 16-34页

作者： Wei Qiao Xingyu Huang ligang feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

Platinum-Ruthenium(PtRu)-based materials are considered the “holy grail” of electrocatalysts for methanol oxidation reaction(MOR) in the fuel cells technique. However,to the best of our knowledge, the exhaustive review report on the advance of PtRu materials for methanol oxidation is rarely summarized for the recent novel achievements. Herein,we summarize and discuss the latest progress of PtRu-based catalysts in MOR. The reaction mechanism of MOR is firstly introduced, and the promotion mechanism is revealed by the relevant activity descriptor, the in-situ spectroscopic analysis and the theoretical calculation. Subsequently, some advanced regulation strategies of PtRu-based catalysts are concluded, including support engineering, morphology design and surface interface regulation. Finally, the challenges and opportunities to improve the MOR performance of PtRubased electrocatalysts are prospected to further promote the widespread application of PtRu-based catalysts in electrocatalytic systems. It is concluded that many efforts are still required to decipher the atomic scale structure-activity relationship and the structural changes of atoms and electrons in the reaction process by advanced strategies and characterization methods. Hopefully, this review can be helpful for novel PtRu-based catalyst development and understanding their correlation to the structure and performance of energy-relevant electrocatalysis.

关键词： Pt-Ru based catalysts electrocatalysis methanol oxidation reaction regulation strategies